Broadband Infrared Spectroscopy of Molecules in Solutions with Two Intrapulse Difference-Frequency-Generated Mid-Infrared Frequency Combs

Mid-infrared (mid-IR) spectroscopy is an incisive tool for studying structures and dynamics of complicated molecules in condensed phases. Developing a compact and broadband mid-IR spectrometer has thus been a long-standing challenge. Here, we show that a highly coherent and broadband mid-IR frequency comb can be generated by using an intrapulse difference-frequency-generation with a train of pulses from a few-cycle pulse Ti:sapphire oscillator. By tightly focusing the oscillator output beam into a single-pass, fan-out-type periodically poled lithium niobate crystal and tilting the orientation of the crystal, we show that a mid-IR frequency comb with more than an octave spectral bandwidth from 1550 cm-1 (46 THz) to 3650 cm-1 (110 THz) and vanishing carrier-envelope-offset phase can be generated. Using two coherent mid-IR frequency combs with different repetition frequencies, we demonstrate that a broadband mid-IR dual-frequency comb spectroscopy of aromatic compounds or amino acids in solutions is feasible. We thus anticipate that researchers will find our mid-IR frequency combs useful for developing ultrafast and broadband linear and nonlinear IR spectroscopy of chemically reactive or biologically important molecules in condensed phases.